Abstract

First time electron spin resonance studies are reported for various isotopomers of GaH2 and HGaCH3. The radicals were generated in neon matrices at 4 K by the ultraviolet photoexcitation of Ga which undergoes insertion reactions with H2 and CH4. Abinitio calculations with a large uncontracted basis and configuration interaction with all single excitations from the spin‐restricted Hartree–Fock configuration gave good agreement with the experimental results and supported the free atom comparison method interpretation of the hyperfineinteractions. A comparison with similar radicals is presented, including BH2, AlH2, HAlCH3, HAlOH, and AlH+.